{"title":"氧官能化的 Mn2C MXene 是一种半导体反铁磁体和高效可见光吸收器","authors":"Jiří Kalmár and František Karlický","doi":"10.1039/D4CP02264E","DOIUrl":null,"url":null,"abstract":"<p >Manganese-based MXenes are promising two-dimensional materials due to the broad palette of their magnetic phases and the possibility of experimental preparation because the corresponding MAX phase was already prepared. Here, we systematically investigated geometrical conformers and spin solutions of oxygen-terminated Mn<small><sub>2</sub></small>C MXene and performed subsequent many-body calculations to obtain reliable electronic and optical properties. Allowing energy-lowering using the correct spin ordering <em>via</em> supercell magnetic motifs is essential for the Mn<small><sub>2</sub></small>CO<small><sub>2</sub></small> system. The stable ground-state Mn<small><sub>2</sub></small>CO<small><sub>2</sub></small> conformation is antiferromagnetic (AFM) with zigzag lines of up and down spins on Mn atoms. The AFM nature is consistent with the parent MAX phase and even the clean depleted Mn<small><sub>2</sub></small>C sheet. Other magnetic states and geometrical conformations are energetically very close, providing state-switching possibilities in the material. Subsequent many-body GW and Bethe–Salpeter equation (BSE) calculations provide indirect semiconductor characteristics of AFM Mn<small><sub>2</sub></small>CO<small><sub>2</sub></small> with a fundamental gap of 2.1 eV (and a direct gap of 2.4 eV), the first bright optical transition at 1.3 eV and extremely strongly bound (1.1 eV) first bright exciton. Mn<small><sub>2</sub></small>CO<small><sub>2</sub></small> absorbs efficiently the whole visible light range and near ultraviolet range (between 10 and 20%).</p>","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":null,"pages":null},"PeriodicalIF":2.9000,"publicationDate":"2024-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Mn2C MXene functionalized by oxygen is a semiconducting antiferromagnet and an efficient visible light absorber†\",\"authors\":\"Jiří Kalmár and František Karlický\",\"doi\":\"10.1039/D4CP02264E\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Manganese-based MXenes are promising two-dimensional materials due to the broad palette of their magnetic phases and the possibility of experimental preparation because the corresponding MAX phase was already prepared. Here, we systematically investigated geometrical conformers and spin solutions of oxygen-terminated Mn<small><sub>2</sub></small>C MXene and performed subsequent many-body calculations to obtain reliable electronic and optical properties. Allowing energy-lowering using the correct spin ordering <em>via</em> supercell magnetic motifs is essential for the Mn<small><sub>2</sub></small>CO<small><sub>2</sub></small> system. The stable ground-state Mn<small><sub>2</sub></small>CO<small><sub>2</sub></small> conformation is antiferromagnetic (AFM) with zigzag lines of up and down spins on Mn atoms. The AFM nature is consistent with the parent MAX phase and even the clean depleted Mn<small><sub>2</sub></small>C sheet. Other magnetic states and geometrical conformations are energetically very close, providing state-switching possibilities in the material. Subsequent many-body GW and Bethe–Salpeter equation (BSE) calculations provide indirect semiconductor characteristics of AFM Mn<small><sub>2</sub></small>CO<small><sub>2</sub></small> with a fundamental gap of 2.1 eV (and a direct gap of 2.4 eV), the first bright optical transition at 1.3 eV and extremely strongly bound (1.1 eV) first bright exciton. Mn<small><sub>2</sub></small>CO<small><sub>2</sub></small> absorbs efficiently the whole visible light range and near ultraviolet range (between 10 and 20%).</p>\",\"PeriodicalId\":99,\"journal\":{\"name\":\"Physical Chemistry Chemical Physics\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":2.9000,\"publicationDate\":\"2024-06-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Physical Chemistry Chemical Physics\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.rsc.org/en/content/articlelanding/2024/cp/d4cp02264e\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Physical Chemistry Chemical Physics","FirstCategoryId":"92","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2024/cp/d4cp02264e","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Mn2C MXene functionalized by oxygen is a semiconducting antiferromagnet and an efficient visible light absorber†
Manganese-based MXenes are promising two-dimensional materials due to the broad palette of their magnetic phases and the possibility of experimental preparation because the corresponding MAX phase was already prepared. Here, we systematically investigated geometrical conformers and spin solutions of oxygen-terminated Mn2C MXene and performed subsequent many-body calculations to obtain reliable electronic and optical properties. Allowing energy-lowering using the correct spin ordering via supercell magnetic motifs is essential for the Mn2CO2 system. The stable ground-state Mn2CO2 conformation is antiferromagnetic (AFM) with zigzag lines of up and down spins on Mn atoms. The AFM nature is consistent with the parent MAX phase and even the clean depleted Mn2C sheet. Other magnetic states and geometrical conformations are energetically very close, providing state-switching possibilities in the material. Subsequent many-body GW and Bethe–Salpeter equation (BSE) calculations provide indirect semiconductor characteristics of AFM Mn2CO2 with a fundamental gap of 2.1 eV (and a direct gap of 2.4 eV), the first bright optical transition at 1.3 eV and extremely strongly bound (1.1 eV) first bright exciton. Mn2CO2 absorbs efficiently the whole visible light range and near ultraviolet range (between 10 and 20%).
期刊介绍:
Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions.
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